Anal Chim Acta67812633.docx
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Anal Chim Acta67812633.docx
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AnalChimActa67812633
Quantitativeanalysisoftriazineherbicidesinenvironmentalsamplesbyusinghighperformanceliquidchromatographyanddiodearraydetectioncombinedwithsecond-ordercalibrationbasedonanalternatingpenaltytrilineardecompositionalgorithm
Yuan-NaLi,Hai-LongWu*,Xiang-DongQing,QuanLi,Shu-FangLi,Hai-YanFu,Yong-JieYu,andRu-QinYu
StateKeyLaboratoryofChemo/BiosensingandChemometrics,CollegeofChemistryandChemicalEngineering,HunanUniversity,Changsha,Hunan410082,PRChina
Correspondingauthor.Tel.:
+86-731-88821818.
Fax:
+86-731-88821818.
E-mail:
hlwu@(H.L.WU).
Abstract
Anovelapplicationofhighperformanceliquidchromatography-diodearraydetection(HPLC-DAD)withsecond-ordercalibrationmethodbasedonanalternatingpenaltytrilineardecomposition(APTLD)algorithmispresentedtoallowaccurateandreliablequantitativeandqualitativeanalysisofatrazine(ATR),ametryn(AME)andprometryne(PRO)insoil,riversedimentandwastewatersamples.Satisfactoryresultsareobtainedalthoughtheelutionandspectralprofilesoftheanalytesareheavilyoverlappedwiththebackgroundinenvironmentalsamples.TheaveragerecoveriesforATR,AMEandPROinsoilsamplesare99.7±1.5,98.4±4.7and97.0±4.4%,respectively;inriversedimentsamplesare100.1±3.2,100.7±3.4and96.4±3.8%,respectively;andinwastewatersamplesare100.1±3.5,101.8±4.2and101.4±3.6%,respectively.Furthermore,theaccuracyandprecisionoftheproposedmethodisinvestigatedbyusingtheellipticaljointconfidenceregion(EJCR)test.Themethodproposedlightsanewavenuetodeterminequantitativelyherbicidesinenvironmentalsampleswithasimplepretreatmentprocedureandprovidesthescientificbasisforanimprovedenvironmentmanagementthroughabetterunderstandingofthewastewater-soil-riversedimentsystemasawhole.
Keywords:
atrazine,ametryn,prometryne,second-ordercalibration,highperformanceliquidchromatography-diodearraydetection,alternatingpenaltytrilineardecompositionalgorithm
1.Introduction
Manualweedingisatraditionalwayforcontrollingweedsinagriculture.Thepracticeisalaborcosting,labor-intensiveandcostlypractice,althoughthe“naturalandcleaning”advantagesareobtained.Alternatively,herbicidesprovidegreatbenefitsforweedcontrolinmodernagriculturedomain.Triazineherbicides,suchasatrazine(ATR),ametryn(AME)andprometryne(PRO),areappliedinagricultureasselectivepre-andpost-emergenceweedcontrolforcorn,rice,wheat,sugarcaneandonionetc.However,ithasbeenestimatedthatonly0.1%ofherbicidesappliedtocropsreachtheirtargets,andalargeproportionremainsintheenvironment[1].Theresiduesoftriazineherbicideshaveattractedgreatconcernworldwideandtheyarealsointhelistofchemicalpollutantsthatneedtobemoreheavilymonitoredowingtotheirwidespreaduseandtheirtoxicity,persistence,cumulationinwater,soilandriversediment.Moreover,atrazine,onenumberofthetriazinefamily,hasalsobeenclassifiedasapossiblehumancarcinogen[2].Ontheotherhand,thequantitativeanalysesofherbicides,inordertomonitor,assessandcontroltheireffectsontheenvironmentandhumanhealth,isoneofthemostimportantfieldsinanalyticalchemistry.
Nowadays,anumberofarticleshavebeenreportedfordeterminationofoneortwotriazineherbicides.Chuangetal.[3]determinedatrazine(ATR)incomplexsamplemediausingimmunoaffinitycolumnchromatography.DeterminationofATRinsoilandwaterusingmercuryfilmelectrodewasreportedbyMalekietal.[4].Themolecularlyimprintedsolid-phaseextraction(MISPE)techniquewasemployedforquantitativeanalysisofametryn(AME)inenvironmentalmatrices[5,6].Determinationofprometryne(PRO)inwaterandsoilbyhigh-performanceliquidchromatography-ultravioletdetector(HPLC-UV)usingcloud-pointextractionwasreportedbyZhouetal.[7].Arangeofanalyticaltechniqueshavebeeninvestigatedfortheirabilitytodetecttwoandmoretriazineherbicides[2,8-11].Whilesometimesmeetingwithsignificantsuccess,thesemethods(ionmobilityspectrometry,HPLC-UVandenzyme-linkedimmunosorbentassay(ELISA))aretimeconsuming,employingdifferentextractionmethodsandgenerallydestroythesamplematerials.AdvantagesanddrawbacksofboththeextractionandchromatographicanalysistothetriazineherbicidesfromenvironmentalsampleswerediscussedbyDeanetal.[12].
Highperformanceliquidchromatographyincombinationwithdiodearraydetection(HPLC-DAD)hasbeenbroadlyusedindeterminationoforganicpollutantsonaccountofitsabilityofanalyzingbothpolarandnonpolarthermodegradablecompounds.However,itisnotpossibletoachieveperfectseparation,eitherbecauseofthecomplexityofthesamplesorbecausefasterchromatographicrunsarepreferred.Sometimes,evenunderthebestexperimentalconditions,theprobabilityofpeakoverlapinchromatographicseparationscanbecomequitesevere,especiallyforthehighlycomplexsamples.Sopriortoquantitativeanalysis,asamplepretreatmentprocedurewouldberequiredbecauseitcanreducetheinterferenceofsamplematrix.However,theextractionprocessesareusuallynotselectiveenough,andoftenanumberofinterferingcomponentsarecoextractedwiththeanalytesofinterest.Aswillbediscussedbelow,amodernapproachtoimprovetheselectivityofanalyticalmethodsistheuseofadvancedsecond-orderchemometricmethods,whichmightlighttoanewavenuetoutilize“mathematicalseparation”toinsteadofthe“physicalorchemicalseparation”ofuncalibratedbackgroundorinterferencesbythechemometricseparationoftheirsignals.Thestrengthofthemethodsisthecapacitytodeterminethecontentoftheanalytesofinteresteveninthepresenceofunknowninterferents,whichisknownas“second-orderadvantage”[13-16].Inrecentdecades,agreatvarietyofsecond-ordercalibrationmethodshavebeenproducedforathree-waydataarray,suchasparallelfactoranalysis(PARAFAC)[17,18],generalizedrankannihilationmethod(GRAM)[19],multivariatecurveresolution-alternatingleastsquares(MCR-ALS)[20],alternatingtrilineardecomposition(ATLD)[21]andalternatingpenaltytrilineardecomposition(APTLD)[22].Theapplicationofsecond-ordercalibrationforHPLC-DADdataarrayhasbeenahottopicinthecurrentchemometricdomain,andhasbeensuccessfullyemployedformanypracticalapplications[21,23-27]andevenforremovalforthree-dimensionalbackgrounddriftincomprehensivetwo-dimensional(2D)liquidchromatographycoupledwithdiodearraydetection(LC×LC-DAD)data[28].
Inthepresentstudy,arapidandeffectivestrategyforsimultaneousdeterminationofATR,AMEandPROinsoil,riversedimentandwastewaterhasbeenproposed,bycombiningHPLC-DADwithsecond-ordercalibrationmethodsbasedontheAPTLDalgorithms.ThemainsuccessofthemethodcanbetoobtaintheATR,AMEandPROconcentrationsincomplexmatricesthatexistingco-elutionofcompoundsandspectraloverlapping.Validationofthemethod,throughassessingitsfiguresofmerit,isacrucialstep,notonlyforassessingthereliabilityoftheresults,butforconsistentlyapplyingthemethodtofuturesituations.Therefore,somestatisticalparametersandfiguresofmeritofAPTLDareevaluated.Theintegratedanalysisofthreetriazineherbicidesofthreedifferentenvironmentalcompartments:
wastewater,soilandriversediment,allowsabetterunderstandingofthewastewater-soil-sedimentsystemasawholeandsummarizingthedistributionoftheherbicidespollution.
2.Experimental
2.1.Reagentsandchemicals
Atrazine(ATR),ametryn(AME)andprometryne(PRO)werepurchasedfromaChinesepharmacyCorporation.StockstandardsolutionsofATR(45.4µgmL-1),AME(36.9µgmL-1)andPRO(35.5µgmL-1)werepreparedinmethanolandstoredat4℃untilused,respectively.MethanolandacetonitrilewereofHPLCgrade.UltrapurewaterwaspreparedusingaMilli-Qwaterpurificationsystem(Millipore,USA).
2.2.InstrumentationandChromatographicconditions
TheHPLCsystemusedwasaLC-20ATliquidchromatographicsystem(ShimadzuCorporation,Japan),whichconsistsofadegasser,fourpumps,amanualinjectorprovidedwitha10lloop,acolumnovenandadiodearraydetector(DAD).TheseparationwascarriedoutinaHypersil-ODSanalyticalcolumn(125mm×4.0mm,5.0m,Shimadzu,Japan).TheLCsolutionsoftwarewasusedforcontrollingtheinstrument,dataacquisition,anddatainterpretation.Inthesamplepreparationprocedure,acentrifuge(Sigma,Germany)andultrasonicinstrument(KQ-250TDB,Jiangsu,China)wereused.
Themobilephasewasisocraticandconsistedofmethanol(85%,v/v)andwater(15%,v/v),pumpedataflowrateof1.0mLmin-1withsampleinjectionvolumeof10l.Thesolventswerefiltereddailythrougha0.45μmcellulosemembranefilterbeforeinjectionintoHPLCcolumn.Thecolumntemperaturewassetat30℃.Photometricdetectionwasperformedintherangeof190-300nm,withaspectralresolutionof1.2nm.Datawasobtainedoveranintegrationperiodof640msperspectrum.IntheMATLABenvironmentallhome-madeprogramswerewrittenandfurtherusedfordataanalysis.
2.3.Samplecollectionandpreparation
ThesoilsamplesandriversedimentsampleswerecollectedfromcroplandandthebankoftheXiangjiangRiverinHunanProvinceofChina,respectively.ThewastewaterwascollectedfromapoolinresidentialareainChangsha,China.Thecollectedsoilsamplesandriversedimentsampleswerestoredinplasticbagsandwedidnotcarryoutanypretreatment.Thesesamplesweredriedatroomtemperature,andgroundwithamortar.Then,100
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